Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Th...Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice.However,the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into allsolid-state thin-film batteries,leading to inexperience in fabricating all-solid-state thin-film Li-S batteries(TFLSBs).Herein,for the first time,TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S(VGsLi2S)composite thin-film cathode,lithium-phosphorous-oxynitride(LiPON)thin-film solid electrolyte,and Li metal anode.Fundamentally eliminating Lipolysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an“unlimited Li”reservoir,which exhibits excellent longterm cycling stability with a capacity retention of 81%for 3,000 cycles,and an exceptional high temperature tolerance up to 60℃.More impressively,VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%.Collectively,this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.展开更多
Lithium phosphorus oxygen nitrogen(LiPON)as solid electrolyte discovered by Bates et al in the 1990s is an important part of all-solid-state thin-film battery(ASSTFB)due to its wide electrochemical stability window an...Lithium phosphorus oxygen nitrogen(LiPON)as solid electrolyte discovered by Bates et al in the 1990s is an important part of all-solid-state thin-film battery(ASSTFB)due to its wide electrochemical stability window and negligible low electronic conductivity.However,the ionic conductivity of LiPON about 2×10^(−6) S cm^(−1) at room temperature is much lower than that of other types of solid electrolytes,which seriously limits the application of ASSTFBs.This review summarizes the research and progress in ASSTFBs based on LiPON,in the solid-state electrolyte of LiPON-derivatives with adjustable chemical compositions of the amorphous structure for the improvement of the ionic conductivity and electrochemical stability,in the critical interface issues between LiPON and electrodes,and in preparation methods for LiPON.This review is helpful for people to understand the interface characteristics and various preparation methods of LiPON in ASSTFBs.The key issues to be addressed concern how to develop solid-state electrolyte films with high conductivity and high-quality interface engineering as well as large-scale preparation technology,so as to realize the practical application of highly integrated ASSTFBs.展开更多
基金supported by National Natural Science Foundation of China(No.U22A20118)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(No.2021ZR146,2021ZZ122)Award Program for Fujian Minjiang Scholar Professorship。
文摘Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice.However,the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into allsolid-state thin-film batteries,leading to inexperience in fabricating all-solid-state thin-film Li-S batteries(TFLSBs).Herein,for the first time,TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S(VGsLi2S)composite thin-film cathode,lithium-phosphorous-oxynitride(LiPON)thin-film solid electrolyte,and Li metal anode.Fundamentally eliminating Lipolysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an“unlimited Li”reservoir,which exhibits excellent longterm cycling stability with a capacity retention of 81%for 3,000 cycles,and an exceptional high temperature tolerance up to 60℃.More impressively,VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%.Collectively,this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.
基金financially supported by the NSAF(Grant No.U20A20336)Tianmu Lake Institute of Advanced Energy Storage Technologies Scientist Studio Program[No.TIES-SS0002].
文摘Lithium phosphorus oxygen nitrogen(LiPON)as solid electrolyte discovered by Bates et al in the 1990s is an important part of all-solid-state thin-film battery(ASSTFB)due to its wide electrochemical stability window and negligible low electronic conductivity.However,the ionic conductivity of LiPON about 2×10^(−6) S cm^(−1) at room temperature is much lower than that of other types of solid electrolytes,which seriously limits the application of ASSTFBs.This review summarizes the research and progress in ASSTFBs based on LiPON,in the solid-state electrolyte of LiPON-derivatives with adjustable chemical compositions of the amorphous structure for the improvement of the ionic conductivity and electrochemical stability,in the critical interface issues between LiPON and electrodes,and in preparation methods for LiPON.This review is helpful for people to understand the interface characteristics and various preparation methods of LiPON in ASSTFBs.The key issues to be addressed concern how to develop solid-state electrolyte films with high conductivity and high-quality interface engineering as well as large-scale preparation technology,so as to realize the practical application of highly integrated ASSTFBs.
